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布朗斯台德酸度在ZSM-5沸石上二甲醚芳构化反应中的作用

The Role of Brønsted Acidity In The Dimethyl Ether Aromatization Over ZSM-5 Zeolites.

作者信息

Golubev Konstantin B, Kolesnichenko Natalia V

机构信息

A.V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences (TIPS RAS), 29 Leninsky Prospect, Moscow, 119991, Russia.

出版信息

Chem Asian J. 2025 Jul;20(13):e202500330. doi: 10.1002/asia.202500330. Epub 2025 May 21.

DOI:10.1002/asia.202500330
PMID:40396683
Abstract

A series of commercial nanosized zeolites and zeolites prepared by in situ seed-induced synthesis with a ZSM-5 structure and a close silica modulus were studied to explore the influence of physicochemical characteristics on the dimethyl ether aromatization and catalyst stability. It was shown that a larger strong Brønsted acidity enhanced the total aromatics formation with an increased light arenes content (especially at elevated WHSV). At low WHSV, excess Brønsted acidity leads to the declined aromatics yield due to its high cracking ability. On the contrary, a higher Lewis acidity and extensive mesoporosity promoted the heavier aromatics production accelerating the coke formation and shortening the catalyst lifetime. An improved aromatization performance and a prolonged durability of the zeolite catalyst were controlled by a balanced Brønsted/Lewis acid site ratio and the ratio of WHSV to acid site concentration.

摘要

研究了一系列商业纳米尺寸沸石以及通过原位晶种诱导合成法制备的具有ZSM-5结构和相近硅铝比的沸石,以探讨物理化学特性对二甲醚芳构化和催化剂稳定性的影响。结果表明,较强的布朗斯台德酸度增强了总芳烃的形成,轻质芳烃含量增加(特别是在较高的重时空速下)。在低重时空速下,过量的布朗斯台德酸度由于其高裂解能力导致芳烃产率下降。相反,较高的路易斯酸度和广泛的介孔率促进了重质芳烃的生成,加速了积炭的形成并缩短了催化剂寿命。通过平衡的布朗斯台德/路易斯酸位比以及重时空速与酸位浓度的比例,可以控制沸石催化剂的芳构化性能的改善和耐久性的延长。

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